Spectroscopic Investigation of the Mechanisms Responsible for the Superior Stability of Hybrid Class 1/Class 2 CO2 Sorbents [electronic resource] : A New Class 4 Category

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Ngôn ngữ: eng

Ký hiệu phân loại: 541.37 Electrochemistry and magnetochemistry

Thông tin xuất bản: Washington, D.C. : Oak Ridge, Tenn. : United States. Office of the Assistant Secretary of Energy for Fossil Energy ; Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy, 2016

Mô tả vật lý: Size: p. 12780-12791 : , digital, PDF file.

Bộ sưu tập: Metadata

ID: 267787

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Hybrid Class 1/Class 2 supported amine CO
2
sorbents demonstrate superior performance under practical steam conditions, yet their amine immobilization and stabilization mechanisms are unclear. Uncovering the interactions responsible for the sorbents? robust features is critical for further improvements and can facilitate practical applications. We employ solid state 
29
Si CP-MAS and 2-D FSLG 
1
H?
13
C CP HETCOR NMR spectroscopies to probe the overall molecular interactions of aminosilane/silica, polyamine [poly(ethylenimine), PEI]/silica, and hybrid aminosilane/PEI/silica sorbents. A unique, sequential impregnation sorbent preparation method is executed in a diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) setup to decouple amine binding mechanisms at the amine?silica interface from those within bulk amine layers. These mechanisms are correlated with each sorbents? resistance to accelerated liquid H
2
O and TGA steam treatments (H
2
O stability) and to oxidative degradation (thermal stability). High percentages of CO
2
capture retained (PCR) and organic content retained (OCR) values after H
2
O testing of N-(3-(trimethoxysilyl)propyl)ethylenediamine (TMPED)/PEI and (3-aminopropyl)trimethoxysilane (APTMS)/PEI hybrid sorbents are associated with a synergistic stabilizing effect of the amine species observed during oxidative degradation (thermal gravimetric analysis-differential scanning calorimetry, TGA-DSC). Solid state NMR spectroscopy reveals that the synergistic effect of the TMPED/PEI mixture is manifested by the formation of hydrogen-bonded PEI?NH
2
��NH
2
?TMPED and PEI?NH
2
��HO?Si/O?Si?O (TMPED, T
2
) linkages within the sorbent. DRIFTS further determines that PEI enhances the grafting of TMPED to silica and that PEI is dispersed among a stable network of polymerized TMPED in the bulk, utilizing H-bonded linkages. These findings provide the scientific basis for establishing a Class 4 category for aminosilane/polyamine/silica hybrid sorbents.

1. 01 coal, lignite, and peat
2. 37 inorganic, organic, physical, and analytical chemistry
3. Amine sorbent
4. Class 4
5. Co2 capture

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Spectroscopic Investigation of the Mechanisms Responsible for the Superior Stability of Hybrid Class 1/Class 2 CO<sub>2</sub> Sorbents [electronic resource] : A New Class 4 Category